Yi Junxuan, Liu Shimei, Li Shulei, He Weichen, Chen Zuxin, Lan Sheng
Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and Devices, School of Optoelectronic Science and Engineering, South China Normal University, Guangzhou 510006, China.
School of Optoelectronic Engineering, Guangdong Polytechnic Normal University, Guangzhou 510665, China.
Nanophotonics. 2025 Mar 14;14(5):601-611. doi: 10.1515/nanoph-2024-0737. eCollection 2025 Mar.
The hybridization of multiple excitons in a heterobilayer composed of two transition metal dichalcogenides (TMDCs) based on strong light-matter interaction is interesting from the viewpoint of both fundamental research and practical application. Here, we investigate numerically and experimentally the hybridization of three excitons in a heterobilayer mediated by the surface plasmon polaritons (SPPs) excited on a thin Au film and the transverse-electric (TE) polarized waves excited on a SiN/Ag heterostructure via photon-exciton coupling. Relying on numerical simulation, we observe anticrossing behaviors in the angle-resolved reflection spectra calculated for MoS/WS/Au and WS/MoS/SiN/Ag heterostructures, which reveal the coupling between the surface wave (SPPs or TE waves) and the multiple excitons in the heterobilayer. In experiments, we employ the oligomers of polystyrene (PS) nanospheres as scatters to transfer the surface waves into far-field radiations. Similarly, we observe anticrossing behaviors in the angle-resolved scattering spectra measured for the oligomers of PS nanospheres. Relying on the coupled oscillator model, we observe Rabi splitting energies of Ω ∼206.79 meV for the SPPs and Ω ∼237.60 meV for the TE waves. Based on the calculated current density distributions and Hopfield coefficients, we demonstrate the hybridization of the three excitons in the WS/MoS heterobilayer mediated by the TE waves. Our findings open new horizons for manipulating light-matter interaction in TMDC heterobilayers and suggest the potential applications of exciton hybridization in energy transfer.
从基础研究和实际应用的角度来看，基于强光与物质相互作用的由两种过渡金属二硫属化物（TMDC）组成的异质双层中多个激子的杂化是很有趣的。在这里，我们通过数值模拟和实验研究了由在薄金膜上激发的表面等离激元极化激元（SPP）和在SiN/Ag异质结构上激发的横电（TE）偏振波通过光子-激子耦合介导的异质双层中三个激子的杂化。依靠数值模拟，我们在为MoS/WS/Au和WS/MoS/SiN/Ag异质结构计算的角分辨反射光谱中观察到反交叉行为，这揭示了表面波（SPP或TE波）与异质双层中多个激子之间的耦合。在实验中，我们使用聚苯乙烯（PS）纳米球的低聚物作为散射体，将表面波转换为远场辐射。同样，我们在为PS纳米球的低聚物测量的角分辨散射光谱中观察到反交叉行为。依靠耦合振子模型，我们观察到SPP的拉比分裂能Ω约为206.79毫电子伏特，TE波的拉比分裂能Ω约为237.60毫电子伏特。基于计算出的电流密度分布和霍普菲尔德系数，我们证明了由TE波介导的WS/MoS异质双层中三个激子的杂化。我们的发现为操纵TMDC异质双层中的光与物质相互作用开辟了新的视野，并暗示了激子杂化在能量转移中的潜在应用。
